Magnetism in cold subducting slabs at mantle transition zone depths.

The Earth's crust-mantle boundary, the Mohorovicic discontinuity, has been traditionally considered to be the interface between the magnetic crust and the non-magnetic mantle1. However, this assumption has been questioned by geophysical observations2,3 and by the identification of magnetic remanence in mantle xenoliths4, which suggest mantle magnetic sources. Owing to their high critical temperatures, iron oxides are the only potential sources of magnetic anomalies at mantle depths5. Haematite (α-Fe2O3) is the dominant iron oxide in subducted lithologies at depths of 300 to 600 kilometres, delineated by the thermal decomposition of magnetite and the crystallization of a high-pressure magnetite phase deeper than about 600 kilometres6. The lack of data on the magnetic properties of haematite at relevant pressure-temperature conditions, however, hinders the identification of magnetic boundaries within the mantle and their contribution to observed magnetic anomalies. Here we apply synchrotron Mössbauer source spectroscopy in laser-heated diamond anvil cells to investigate the magnetic transitions and critical temperatures in Fe2O3 polymorphs7 at pressures and temperatures of up to 90 gigapascals and 1,300 kelvin, respectively. Our results show that haematite remains magnetic at the depth of the transition zone in the Earth's mantle in cold or very cold subduction geotherms, forming a frame of deep magnetized rocks in the West Pacific region. The deep magnetic sources spatially correlate with preferred paths of the Earth's virtual geomagnetic poles during reversals8 that might not reflect the geometry of the transitional field. Rather, the paths might be an artefact caused by magnetized haematite-bearing rocks in cold subducting slabs at mid-transition zone depths. Such deep sources should be taken into account when carrying out inversions of the Earth's geomagnetic data9, and especially in studies of planetary bodies that no longer have a dynamo10, such as Mars.

The validity of an experiment testing the influence of acceleration on time dilation using a rotating Mössbauer absorber and a Synchrotron Mössbauer Source.

Three experiments are reviewed, performed (in 2014-2016) at ID18 of ESRF to measure the influence of acceleration on time dilation by measuring the relative shift between the absorption lines of two states of the same rotating absorber with accelerations anti-parallel and parallel to the incident beam. Statistically significant data for rotation frequencies up to 510 Hz in both directions of rotation were collected. For each run with high rotation, a stable statistically significant `vibration-free' relative shift between the absorption lines of the two states was measured. This may indicate the influence of acceleration on time dilation. However, the measured relative shift was also affected by the use of a slit necessary to focus the beam to the axis of rotation to a focal spot of sub-micrometre size. The introduction of the slit broke the symmetry in the absorption lines due to the nuclear lighthouse effect and affected the measured relative shift, preventing to claim conclusively the influence of acceleration on time dilation. Assuming that this loss of symmetry is of first order, the zero value of the relative shift, corrected for this loss, falls always within the experimental error limits, as predicted by Einstein's clock hypothesis. The requirements and an indispensable plan for a conclusive experiment, once the improved technology becomes available, is presented. This will be useful to future experimentalists wishing to pursue this experiment or a related rotor experiment involving a Mössbauer absorber and a synchrotron Mössbauer source.

Advances in testing the effect of acceleration on time dilation using a synchrotron Mössbauer source.

New results, additional techniques and know-how acquired, developed and employed in a recent HC-1898 experiment at the Nuclear Resonance Beamline ID18 of ESRF are presented, in the quest to explore the acceleration effect on time dilation. Using the specially modified Synchrotron Mössbauer Source and KB-optics together with a rotating single-line semicircular Mössbauer absorber on the rim of a specially designed rotating disk, the aim was to measure the relative spectral shift between the spectra of two states when the acceleration of the absorber is anti-parallel and parallel to the source. A control system was used for the first time and a method to quantify the effects of non-random vibrations on the spectral shift was developed. For several runs where the effect of these vibrations was negligible, a stable statistically significant non-zero relative shift was observed. This suggests the influence of acceleration on time.

Erratum: Lattice Dynamics of EuO: Evidence for Giant Spin-Phonon Coupling [Phys. Rev. Lett. 116, 185501 (2016)].

This corrects the article DOI: 10.1103/PhysRevLett.116.185501.

Anomalous Lattice Dynamics of EuSi_{2} Nanoislands: Role of Interfaces Unveiled.

We report a systematic lattice dynamics study of EuSi_{2} films and nanoislands by in situ nuclear inelastic scattering on ^{151}Eu and ab initio theory. The Eu-partial phonon density of states of the nanoislands exhibits anomalous excess of phonon states at low and high energies, not present in the bulk and at the EuSi_{2}(001) surface. We demonstrate that atomic vibrations along the island-substrate interface give rise to phonon states both at low and high energies, while atomic vibrations across the island-island interface result in localized high-energy phonon modes.

Lattice Dynamics of EuO: Evidence for Giant Spin-Phonon Coupling.

Comprehensive studies of lattice dynamics in the ferromagnetic semiconductor EuO have been performed by a combination of inelastic x-ray scattering, nuclear inelastic scattering, and ab initio calculations. A remarkably large broadening of the transverse acoustic phonons was discovered at temperatures above and below the Curie temperature T_{C}=69 K. This result indicates a surprisingly strong momentum-dependent spin-phonon coupling induced by the spin dynamics in EuO.

Synchrotron radiation Mössbauer spectra of a rotating absorber with implications for testing velocity and acceleration time dilation.

Many Mössbauer spectroscopy (MS) experiments have used a rotating absorber in order to measure the second-order transverse Doppler (TD) shift, and to test the validity of the Einstein time dilation theory. From these experiments, one may also test the clock hypothesis (CH) and the time dilation caused by acceleration. In such experiments the absorption curves must be obtained, since it cannot be assumed that there is no broadening of the curve during the rotation. For technical reasons, it is very complicated to keep the balance of a fast rotating disk if there are moving parts on it. Thus, the Mössbauer source on a transducer should be outside the disk. Friedman and Nowik have already predicted that the X-ray beam finite size dramatically affects the MS absorption line and causes its broadening. We provide here explicit formulas to evaluate this broadening for a synchrotron Mössbauer source (SMS) beam. The broadening is linearly proportional to the rotation frequency and to the SMS beam width at the rotation axis. In addition, it is shown that the TD shift and the MS line broadening are affected by an additional factor assigned as the alignment shift which is proportional to the frequency of rotation and to the distance between the X-ray beam center and the rotation axis. This new shift helps to align the disk's axis of rotation to the X-ray beam's center. To minimize the broadening, one must focus the X-ray on the axis of the rotating disk and/or to add a slit positioned at the center, to block the rays distant from the rotation axis of the disk. Our experiment, using the (57)Fe SMS, currently available at the Nuclear Resonance beamline (ID18) at the ESRF, with a rotating stainless steel foil, confirmed our predictions. With a slit installed at the rotation axis (reducing the effective beam width from 15.6 µm to 5.4 µm), one can measure a statistically meaningful absorption spectrum up to 300 Hz, while, without a slit, such spectra could be obtained up to 100 Hz only. Thus, both the broadening and the alignment shift are very significant and must be taken into consideration in any rotating absorber experiment. Here a method is offered to measure accurately the TD shift and to test the CH.

Phonons in Ultrathin Oxide Films: 2D to 3D Transition in FeO on Pt(111).

The structural and magnetic properties of ultrathin FeO(111) films on Pt(111) with thicknesses from 1 to 16 monolayers (MLs) were studied using the nuclear inelastic scattering of synchrotron radiation. A distinct evolution of vibrational characteristics with thickness, revealed in the phonon density of states (PDOS), shows a textbook transition from 2D to 3D lattice dynamics. For the thinnest films of 1 and 2 ML, the low-energy part of the PDOS followed a linear ∝E dependence in energy that is characteristic for two-dimensional systems. This dependence gradually transforms with thickness to the bulk ∝E^{2} relationship. Density-functional theory phonon calculations perfectly reproduced the measured 1-ML PDOS within a simple model of a pseudomorphic FeO/Pt(111) interface. The calculations show that the 2D PDOS character is due to a weak coupling of the FeO film to the Pt(111) substrate. The evolution of the vibrational properties with an increasing thickness is closely related to a transient long-range magnetic order and stabilization of an unusual structural phase.

Nuclear forward scattering of synchrotron radiation by 99Ru.

We measured nuclear forward scattering spectra utilizing the (99)Ru transition, 89.571(3) keV, with a notably mixed E2/M1 multipolarity. The extension of the standard evaluation routines to include mixed multipolarity allows us to extract electric and magnetic hyperfine interactions from (99)Ru-containing compounds. This paves the way for several other high-energy Mössbauer transitions, E ∼ 90 keV. The high energy of such transitions allows for operando nuclear forward scattering studies in real devices.

Role of disorder in the thermodynamics and atomic dynamics of glasses.

We measured the density of vibrational states (DOS) and the specific heat of various glassy and crystalline polymorphs of SiO2. The typical (ambient) glass shows a well-known excess of specific heat relative to the typical crystal (α-quartz). This, however, holds when comparing a lower-density glass to a higher-density crystal. For glassy and crystalline polymorphs with matched densities, the DOS of the glass appears as the smoothed counterpart of the DOS of the corresponding crystal; it reveals the same number of the excess states relative to the Debye model, the same number of all states in the low-energy region, and it provides the same specific heat. This shows that glasses have higher specific heat than crystals not due to disorder, but because the typical glass has lower density than the typical crystal.

The dynamics of the non-heme iron in bacterial reaction centers from Rhodobacter sphaeroides.

We investigate the dynamical properties of the non-heme iron (NHFe) in His-tagged photosynthetic bacterial reaction centers (RCs) isolated from Rhodobacter (Rb.) sphaeroides. Mössbauer spectroscopy and nuclear inelastic scattering of synchrotron radiation (NIS) were applied to monitor the arrangement and flexibility of the NHFe binding site. In His-tagged RCs, NHFe was stabilized only in a high spin ferrous state. Its hyperfine parameters (IS=1.06±0.01mm/s and QS=2.12±0.01mm/s), and Debye temperature (θ(D0)~167K) are comparable to those detected for the high spin state of NHFe in non-His-tagged RCs. For the first time, pure vibrational modes characteristic of NHFe in a high spin ferrous state are revealed. The vibrational density of states (DOS) shows some maxima between 22 and 33meV, 33 and 42meV, and 53 and 60meV and a very sharp one at 44.5meV. In addition, we observe a large contribution of vibrational modes at low energies. This iron atom is directly connected to the protein matrix via all its ligands, and it is therefore extremely sensitive to the collective motions of the RC protein core. A comparison of the DOS spectra of His-tagged and non-His-tagged RCs from Rb. sphaeroides shows that in the latter case the spectrum was overlapped by the vibrations of the heme iron of residual cytochrome c(2), and a low spin state of NHFe in addition to its high spin one. This enabled us to pin-point vibrations characteristic for the low spin state of NHFe.

Hyperfine splitting and room-temperature ferromagnetism of Ni at multimegabar pressure.

Magnetic and elastic properties of Ni metal have been studied up to 260 GPa by nuclear forward scattering of synchrotron radiation with the 67.4 keV Mössbauer transition of 61Ni. The observed magnetic hyperfine splitting confirms the ferromagnetic state of Ni up to 260 GPa, the highest pressure where magnetism in any material has been observed so far. Ab initio calculations reveal that the pressure evolution of the hyperfine field, which features a maximum in the range of 100 to 225 GPa, is a relativistic effect. The Debye energy obtained from the Lamb-Mössbauer factor increases from 33 meV at ambient pressure to 60 meV at 100 GPa. The change of this energy over volume compression is well described by a Grüneisen parameter of 2.09.

Importance of correlation effects in hcp iron revealed by a pressure-induced electronic topological transition.

We discover that hcp phases of Fe and Fe(0.9)Ni(0.1) undergo an electronic topological transition at pressures of about 40 GPa. This topological change of the Fermi surface manifests itself through anomalous behavior of the Debye sound velocity, c/a lattice parameter ratio, and Mössbauer center shift observed in our experiments. First-principles simulations within the dynamic mean field approach demonstrate that the transition is induced by many-electron effects. It is absent in one-electron calculations and represents a clear signature of correlation effects in hcp Fe.

Equivalence of the boson peak in glasses to the transverse acoustic van Hove singularity in crystals.

We compare the atomic dynamics of the glass to that of the relevant crystal. In the spectra of inelastic scattering, the boson peak of the glass appears higher than the transverse acoustic (TA) singularity of the crystal. However, the density of states shows that they have the same number of states. Increasing pressure causes the transformation of the boson peak of the glass towards the TA singularity of the crystal. Once corrected for the difference in the elastic medium, the boson peak matches the TA singularity in energy and height. This suggests the identical nature of the two features.

Experimental evidence of mosaic structure in strongly supercooled molecular liquids.

When a liquid is cooled to produce a glass its dynamics, dominated by the structural relaxation, become very slow, and at the glass-transition temperature Tg its characteristic relaxation time is about 100 s. At slightly elevated temperatures (~1.2 Tg) however, a second process known as the Johari-Goldstein relaxation, ßJG, decouples from the structural one and remains much faster than it down to Tg. While it is known that the ßJG-process is strongly coupled to the structural relaxation, its dedicated role in the glass-transition remains under debate. Here we use an experimental technique that permits us to investigate the spatial and temporal properties of the ßJG relaxation, and give evidence that the molecules participating in it are highly mobile and spatially connected in a system-spanning, percolating cluster. This correlation of structural and dynamical properties provides strong experimental support for a picture, drawn from theoretical studies, of an intermittent mosaic structure in the deeply supercooled liquid phase.

Noncollinear magnetization structure at the thickness-driven spin-reorientation transition in epitaxial Fe films on W(110).

An in-plane spin-reorientation transition occurring during the growth of epitaxial Fe films on W(110) was studied in situ by using the nuclear resonant scattering of synchrotron radiation. The spin-reorientation transition originates at the Fe/W(110) interface and proceeds via a noncollinear spin structure resembling a planar domain wall that propagates towards the surface with increasing film thickness.

Wave theory of focusing monochromator of synchrotron radiation.

The concept of a focusing monochromator with high energy resolution is presented. Different from conventional optical schemes, the device exploits not the angular but the spatial dispersion of synchrotron radiation. The wave theory of the monochromator is developed; it shows that the monochromator can reach an energy resolution of about 0.1 meV without significant loss of the spectral density of synchrotron radiation.

Portable laser-heating system for diamond anvil cells.

The diamond anvil cell (DAC) technique coupled with laser heating has become the most successful method for studying materials in the multimegabar pressure range at high temperatures. However, so far all DAC laser-heating systems have been stationary: they are linked either to certain equipment or to a beamline. Here, a portable laser-heating system for DACs has been developed which can be moved between various analytical facilities, including transfer from in-house to a synchrotron or between synchrotron beamlines. Application of the system is demonstrated in an example of nuclear inelastic scattering measurements of ferropericlase (Mg(0.88)Fe(0.12))O and h.c.p.-Fe(0.9)Ni(0.1) alloy, and X-ray absorption near-edge spectroscopy of (Mg(0.85)Fe(0.15))SiO(3) majorite at high pressures and temperatures. Our results indicate that sound velocities of h.c.p.-Fe(0.9)Ni(0.1) at pressures up to 50 GPa and high temperatures do not follow a linear relation with density.

A microscopic look at the Johari-Goldstein relaxation in a hydrogen-bonded glass-former.

Understanding the glass transition requires getting the picture of the dynamical processes that intervene in it. Glass-forming liquids show a characteristic decoupling of relaxation processes when they are cooled down towards the glassy state. The faster (ßJG) process is still under scrutiny, and its full explanation necessitates information at the microscopic scale. To this aim, nuclear γ-resonance time-domain interferometry (TDI) has been utilized to investigate 5-methyl-2-hexanol, a hydrogen-bonded liquid with a pronounced ßJG process as measured by dielectric spectroscopy. TDI probes in fact the center-of-mass, molecular dynamics at scattering-vectors corresponding to both inter- and intra-molecular distances. Our measurements demonstrate that, in the undercooled liquid phase, the ßJG relaxation can be visualized as a spatially-restricted rearrangement of molecules within the cage of their closest neighbours accompanied by larger excursions which reach out at least the inter-molecular scale and are related to cage-breaking events. In-cage rattling and cage-breaking processes therefore coexist in the ßJG relaxation.

Tracking the Connection between Disorder and Energy Landscape in Glasses Using Geologically Hyperaged Amber.

Fossil amber offers the unique opportunity to investigate an amorphous material that has been exploring its energy landscape for more than 110 million years of natural aging. By applying different X-ray scattering methods to amber before and after annealing the sample to erase its thermal history, we identify a link between the potential energy landscape and the structural and vibrational properties of glasses. We find that hyperaging induces a depletion of the vibrational density of states in the terahertz region, also ruling the sound dispersion and attenuation properties of the corresponding acoustic waves. Critically, this is accompanied by a densification with structural implications different in nature from that caused by hydrostatic compression. Our results, rationalized within the framework of fluctuating elasticity theory, reveal how upon approaching the bottom of the potential energy landscape (9% decrease in the fictive temperature) the elastic matrix becomes increasingly less disordered (6%) and longer-range correlated (22%).